The Green Recycling and Reuse of the Spent Lithium-Ion Battery with Nickel Cobalt Manganate as the Cathode

Abstract

With the wide use of lithium-ion batteries (LIBs), the amount of spent LIBs is also increasing rapidly. So it is necessary to recycle and reuse end-of-life batteries. However, the traditional hydrometallurgy recycling strategy with the coprecipitation process inevitably produces high-concentration Na2SO4 wastewater (3.4 ton Na2SO4 waste will be generated by producing 1 ton ternary precursor). To solve this problem, we develop a green closed-loop recycling method for spent LIBs cathode materials which combines electrolysis and hydrometallurgy technology. Pure sulfuric acid and sodium hydroxide solutions are prepared by Na2SO4 electrolysis, and they are the main raw materials for the leaching and resynthesis of waste cathodes, respectively. Under the best leaching conditions, the valuable metals are almost completely leached, and Li2CO3 and precursor Ni0.8Co0.1Mn0.1(OH)2 are precipitated from the leachate. At the appropriate temperature and ratio, the recovered Li2CO3 and the precursor are calcined together to regenerate a new cathode material LiNi0.8Co0.1Mn0.1O2. The regenerated cathode material has good electrochemical performance. The final Na2SO4 solution can be electrolyzed again after simple treatment to achieve recycling. This recycling method reduces the consumption of additional reagents, produces no waste, and has economic benefits. It provides a new path for the recycling of spent LIBs and promotes the sustainable development of lithium-ion batteries.

Keywords: Spent lithium-ion battery, electrolysis, recycle, Environmentally friendly